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In situ thermoresponsive supramolecular assembly for switchable circularly polarized luminescence

Science China Chemistry 2024年第7期67卷 2362-2372页

作者： Menghan Pan Gong Zhang Haotian Ma Xiaoxiao Cheng Jieai Li Wei Zhang state and local joint engineering laboratory for novel functional polymeric materials Jiangsu Engineering Laboratory of Novel Functional Polymeric MaterialsSuzhou Key Laboratory of Macromolecular Design and Precision SynthesisCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123China School of Chemical and Environmental engineering Anhui Polytechnic UniversityWuhu 241000China

The dynamic regulation of circularly polarized luminescence(CPL)holds profound significance in various fields,such as highlevel information storage and encryption.Here we developed a chiral amphiphilic molecule,CPSB-GLU-PEG350(CGP),composed of aggregation-induced emission(AIE)chromophores(Z)-4-(1-cyano-2-phenylvinyl)benzoic acid(CPSB),a chiral linker Glutamic acid and polyethylene glycol(PEG)thermoresponsive segments.Within the self-assembled supramolecular system formed by CGP,we have achieved in-situ temperature-responsive chiral structures,facilitating the thermal control switch of the CPL signal.Molecular dynamics simulations demonstrate the distinct behaviors of AIE and PEG units during the temperature-variable assembly process.Furthermore,by co-assembling achiral dye molecules with CGP,we have expanded the color range of the temperature-responsive CPL assembly system in situ and confirmed the occurrence of circularly polarizedF?rster resonance energy transfer(C-FRET)phenomenon in this process,which successfully enriched the strategies for in-situ CPL control in aqueous phases.In addition,the contactless radiative energy transfer of CPL can also be realized in this system,exhibiting more flexible temperature regulation of the CPL signal.This study provides a convenient and universal strategy for the construction of dynamically smart chiroptical materials.

关键词： circularly polarized luminescence in-situ thermoresponsive supramolecular assembly energy transfer

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Persistent radical anion of perylene dianhydride:an emerging metal-free photocatalyst for near-infrared photocontrolled RAFT polymerization

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Science China Chemistry 2024年第2期67卷 677-686页

作者： Haitao Zhao Guoqing Bian Xiang Xu Weiwei He Lifen Zhang Zhenping Cheng state and local joint engineering laboratory for novel functional polymeric materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and ApplicationSuzhou Key Laboratory of Macromolecular Design and Precision SynthesisCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou215123China

Developing a new type of photocatalyst(PC) and catalytic mechanism for near-infrared(NIR) photocontrolled reversibledeactivation radical polymerization(RDRP) system is charming but challenging.Herein,a novel PC of the persistent radical anion(PRA)(possessing the properties of both radical and anion) was developed for NIR photocontrolled reversible additionfragmentation chain transfer(RAFT) polymerization,enabling successful polymerization while gaining a deep insight into the mechanism of photo-induced electron transfer RAFT(PET-RAFT) polymerization.Different from the conventional and wellaccepted reductive quenching(RQ) pathway,in which the radical anion intermediates of PCs(PCs^(·-)) must be generated in an excited state(ES),here,the PRA(3,4,9,10-perylenetetracarboxylic dianhydride radical anion(PTCDA^(·-))) could generate conveniently in situ in the ground state(GS) and subsequently serve as highly efficient PC in the NIR region(740–850 nm).The successful implementation of this strategy elucidates the peculiar role played by light and the real way of electron transfer behaviors.In fact,the transfer of a single electron from PRA to chain transfer agent(CTA) and cleavage of the C–S bonds is a process from ES to GS,rather than always from GS(PCs^(·-)) to GS(CTA) in the RQ pathway as is well known to all.In addition,the excellent spatial-temporal control and powerful penetration ability of the NIR light were also confirmed by this PRAcatalyzed polymerization system.

关键词： photocatalyst persistent radical anion(PRA) near-infrared(NIR)light reversible-deactivation radical polymerization(RDRP) photo-induced electron transfer RAFT(PET-RAFT)polymerization

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A nanoplatform with oxygen self-supplying and heat-sensitizing capabilities enhances the efficacy of photodynamic therapy in eradicating multidrug-resistant biofilms

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Journal of materials Science & Technology 2024年第2期169卷 209-219页

作者： Haixin Zhang Yi Zou Kunyan Lu Yan Wu Yuancheng Lin Jingjing Cheng Chunxia Liu Hong Chen Yanxia Zhang Qian Yu state and local joint engineering laboratory for novel functional polymeric materials College of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123China Department of Cardiovascular Surgery of the First Affiliated Hospital and Institute for Cardiovascular Science Suzhou Medical College of Soochow UniversitySoochow UniversitySuzhou 215007China

Bacterial biofilms,especially those caused by multidrug-resistant bacteria,have emerged as one of the greatest dangers to global public health.The acceleration of antimicrobial resistance to conventional an-tibiotics and the severe lack of new drugs necessitates the development of novel agents for biofilm eradication.Photodynamic therapy(PDT)is a promising non-antibiotic method for treating bacterial infections.However,its application in biofilm eradication is hampered by the hypoxic microenvironment of biofilms and the physical protection of extracellular polymeric substances.In this study,we develop a composite nanoplatform with oxygen(O_(2))self-supplying and heat-sensitizing capabilities to improve the PDT efficacy against biofilms.CaO_(2)/ICG@PDA nanoparticles(CIP NPs)are fabricated by combining calcium peroxide(CaO_(2))with the photosensitizer indocyanine green(ICG)via electrostatic interactions,followed by coating with polydopamine(PDA).The CIP NPs can gradually generate O_(2)in response to the acidic microenvironment of the biofilm,thereby alleviating its hypoxic state.Under near-infrared(NIR)irradiation,the nanoplatform converts O_(2)into a significant amount of singlet oxygen(^(1)O_(2))and heat to eradicate biofilm.The generated heat enhances the release of O_(2),accelerates the generation of^(1)O_(2)in PDT,increases cell membrane permeability,and increases bacterial sensitivity to^(1)O_(2).This nanoplatform significantly improves the efficacy of PDT in eradicating biofilm-dwelling bacteria without fostering drug resistance.Experiments on biofilm eradication demonstrate that this nanoplatform can eradicate over 99.9999%of methicillin-resistant Staphylococcus aureus(MRSA)biofilms under 5-min NIR irradiation.Notably,these integrated advantages enable the system to promote the healing of MRSA biofilm-infected wounds with negligible toxicity in vivo,indicating great promise for overcoming the obstacles associated with bacterial biofilm eradication.

关键词： Bacterial biofilm Multidrug-resistant bacteria Photodynamic therapy Oxygen supplying Photothermal therapy

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Manipulating the Phase Transition Behavior of Dual Temperature-Responsive Block Copolymers by Adjusting Composition and Sequence

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Chinese Journal of Polymer Science 2024年第2期42卷 176-187,I0006页

作者： Zhi Zou Xiang Xu Hai-Tao Zhao Jian-Nan Cheng Wei-Wei He Li-Fen Zhang Zhen-Ping Cheng Suzhou key laboratory of Macromolecular Design and Precision Synthesis Jiangsu Key Laboratory of Advanced Functional Polymer Design and ApplicationState and Local Joint Engineering Laboratory for Novel Functional Polymeric MaterialsCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou215123China state Key laboratory of Radiation Medicine and Protection School for Radiological and Interdisciplinary Sciences(RAD-X)and Collaborative Innovation Center of Radiation Medicine of JiangsuSoochow UniversitySuzhou215123China

Temperature-responsive polymers have garnered significant attention due to their ability to respond to external stimuli.In this work,dual temperature-responsive block copolymers are synthesized via reversible addition-fragmentation chain transfer polymerization(RAFT)polymerization utilizing zwitterionic monomer methacryloyl ethyl sulfobetaine(SBMA) and N-isopropyl acrylamide(NIPAAm) as monomers.The thermal responsive behaviors can be easily modulated by incorporating additional hydrophobic monomer benzyl acrylate(BN) or hydrophilic monomer acrylic acid(AA),adjusting concentration or pH,or varying the degree of polymerization of the block chain segments.The cloud points of the copolymers are determined by UV-Vis spectrophotometry,and these copolymers exhibit both controlled upper and lower critical solu bility temperatures(LCST and UCST) in aqueous solution.This study analyzes and summarizes the influencing factors of dual temperature responsive block copolymers by exploring the effects of various conditions on the phase transition temperature of temperature-sensitive polymers to explore the relationship between their properties and environment and structure to make them more selective in terms of temperature application range and regulation laws.It is very interesting that the introduction of poly-acrylic acid(PAA) segments in the middle of di-block copolymer PSBMA_(55)-b-PNIPAAm_(80) to form PSBMA_(55)-b-PAA_(x)-b-PNIPAAm_(80) results in a reversal of temperature-responsive behaviors from 'U'(LCST UCST) type,while the copolymer PSBMA_(55)-b-P(NIPAAm_(80)-co-AA_(x)) not.This work provides a clue for tuning the phase transition behavior of polymers for manufacture of extreme smart materials.

关键词： Temperature responsive polymers High critical solubility temperature(UCST) Low critical solubility temperature(LCST) Block copolymers

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Thienothiophene-centered ladder-type π-systems that feature distinct quinoidal π-extension

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Chinese Chemical Letters 2024年第5期35卷 249-253页

作者： Jiaxiang Guo Zeyi Li Tianyu Zhang Xinyu Tian Yue Wang Chuandong Dou state Key laboratory of Supramolecular Structure and materials College of ChemistryJilin UniversityChangchun 130012China Jiangsu engineering laboratory of novel functional polymeric materials Soochow UniversitySuzhou 215123China

Quinoidalπ-conjugated structures,a kind of fundamental subunits for organicπ-systems,may produce some intriguing optical,electronic and magnetic properties of polycyclic hydrocarbons(PHs).Herein,we report two thienothiophene-centered ladder-type polycyclic molecules(1 and 2),which possess one quinoidal thienothiophene moiety and two para-quinodimethane(p-QDM)subunits,respectively.As theoretically and experimentally studied,while 1 is a fully closed-shell molecule,2 owns an open-shell structure along with partial contribution of tetraradical state that is induced by the resonance of p-QDM.Moreover,although 2 has a largerπ-conjugated skeleton and open-shell electronic state,it exhibits larger bandgap and blue-shifted absorption.On the other hand,the reversible oxidation activity of 1 enables the preparation of its dication 1^(2+),and the studies on its single-crystal and aromatic structures demonstrate that its two positive charges are delocalized onto the oxygen atoms,thus achieving fullyπ-extended structure and near-infrared absorption.This study not only gains insight into quinoidalπ-subunits,but also provides an important basis for the development of antiaromatic and open-shellπ-electron materials.

关键词： Thienothiophene Quinoidal conjugation Open-shell structure Aromaticity Photophysical properties

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Recent Advances in Asymmetric Structural Composites for Excellent Electromagnetic Interference Shielding: A Review

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Chinese Journal of Polymer Science 2024年第6期42卷 693-710页

作者： Ying Zhou Bai Xue Lan Xie Chang-Mei Wu Qiang Zheng Department of Polymer materials and engineering College of Materials and Metallurgy Guizhou University National engineering Research Center for Compounding and Modification of Polymer materials National and Local Joint Engineering Research Center for Functional Polymer Membrane Materials and Membrane Processes state Key laboratory of Public Big Data Guizhou University Department of Polymer Science and engineering Zhejiang University

Since electromagnetic pollution is detrimental to human health and the environment, numerous efforts have been successively made to achieve excellent electromagnetic interference shielding effectiveness(EMI SE) via designing the hierarchical structures for electromagnetic interference(EMI) shielding polymer composites. Among the plentiful structures, the asymmetric structures are currently a hot spot, principally categorizing into multi-layered, porous, fibrous, and segregated asymmetric structures, which endows the high EMI shielding performance for polymer composites incorporated with magnetic, conductive, and/or dielectric micro/nano-fillers, due to the “absorption-reflection-reabsorption” shielding mechanism. Therefore, this review provides the retrospection and summary of the efforts with respect to abundant asymmetric structures and multifunctional micro/nano-fillers for enhancing EMI shielding properties, which is conducive to the booming development of polymeric EMI shielding materials for the promising prospect in modern electronics and 5-generation(5G) technology.

关键词： Asymmetric structure Microano functional filler Polymer composite Electromagnetic interference shielding

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MOF and its derivative materials modified lithium-sulfur battery separator:a new means to improve performance

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Rare Metals 2024年第6期43卷 2418-2443页

作者： Rong-Wei Huang Yong-Qi Wang Dan You Wen-Hao Yang Bin-Nan Deng Fei Wang Yue-Jin Zeng Yi-Yong Zhang Xue Li National local joint engineering Research Center for Lithium-Ion Batteries and materials Preparation Technology Key Laboratory of Advanced Batteries Materials of Yunnan ProvinceFaculty of Metallurgical and Energy EngineeringKunming University of Science and Technology state Key laboratory of Physical Chemistry of Solid Surfaces Collaborative Innovation Centre of Chemistry for Energy MaterialsState-Province Joint Engineering Laboratory of Power Source Technology for New Energy VehicleEngineering Research Center of Electrochemical TechnologyMinistry of EducationCollege of Chemistry and Chemical EngineeringXiamen University

In recent years,lithium-sulfur batteries（LSBs）are considered as one of the most promising new generation energies with the advantages of high theoretical speeific capacity of sulfur(1675 mAh·g-1),abundant sulfur resources,and environmental friendliness storage technologies,and they are receiving wide attention from the industry.However,the problems of the shuttle effect and lithium dendrite growth in LSBs have limited their practical application,so there is a need to find ways to solve these problems.It is an excellent choice to use novel materials to modify battery materials.Among those novel materials,the metal-organic framework（MOF） has the properties of regular pores and controllable structure.When applied as a positive electrode and diaphragm,it can restrain the shuttle effect and lithium dendrite growth,especially since it shows excellent performance in diaphragm modification.Therefore,various design strategies and synthesis methods of MOF-modified separators are reviewed in this paper,and the applications of MOF in LSBs separators in different forms are introduced,including the composite of MOF and carbon-based materials,the compounding of MOF and polymer,self-carbonization to form MOF-derived materials.At the same time,different characterization techniques are systematically reviewed to obtain the physical and chemical properties of MOF particles and the working mechanism of MOF-modified diaphragm,which provides a basis for further research in this field.Finally,some future research trends and directions are put forward to fully tap the future commercial potential of MOF-modified diaphragm in LSBs.

关键词： MOF Lithium–sulfur battery Modified diaphragms Design strategies Prospect Characterization

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Efficient and stable organic solar cells enabled by a poly(carbazole phosphonic acid)hole transporter

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Science China Chemistry 2024年第6期67卷 1941-1945页

作者： Zhijun Ren Siwei Luo Xiaoyu Shi Yunjie Dou Tianxiao Liu Lingyuan Wang Kwok Kiu Tsang Feifei Wang Yu Zhao Yangyang Liu Xiaodong Hu Xiaoxiao Peng Wei Liu He Yan Shangshang Chen state Key laboratory of Coordination Chemistry MOE Key Laboratory of High Performance Polymer Materials&TechnologySchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing210023China Department of Chemistry Guangdong-Hong Kong-Macao Joint Laboratory of Optoelectronic and Magnetic Functional MaterialsEnergy Institute and Hong Kong Branch of Chinese NationalEngineering Research Center for Tissue Restoration and ReconstructionHong Kong University of Science and TechnologyHong Kong999077China

Conventional self-assembled monolayer(SAM)hole transporters in organic solar cells(OSCs)generally suffer from poor uniformity and limited thickness tolerance,hindering their large-scale production.To overcome these limitations,we introduce a novel polymeric hole transporter synthesized by polymerizing carbazole phosphonic acid(PACz).The resultant Poly-2PACz material exhibits exceptional conductivity,high tolerance for variations in layer thickness,and improved film uniformity compared with conventional SAMs.Consequently,the OSCs utilizing Poly-2PACz achieve a remarkable power conversion efficiency of 19.1%and a high fill factor of 81.2%,surpassing the devices based on 2PACz.Moreover,Poly-2PACz-based OSCs demonstrate excellent operational stability,retaining over 80%of their initial efficiency after 1,400 h of continuous light exposure in ambient conditions.This work presents a novel strategy for designing hole transporters,paving the way for more efficient and stable OSCs.

关键词： organic solar cells hole transporters poly(carbazole phosphonic acid) stability

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Self-derivation and reconstruction of silver nanoparticle reinforced cobalt-nickel bimetallic hydroxides through interface engineering for overall water splitting

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Journal of Energy Chemistry 2024年第3期90卷 590-599,I0013页

作者： Yan Li Jie Han Weiwei Bao Junjun Zhang Taotao Ai Mameng Yang Chunming Yang Pengfei Zhang National and local joint engineering laboratory for Slag Comprehensive Utilization and Environmental Technology School of Materials Science and EngineeringShaanxi University of TechnologyHanzhong 723000ShaanxiChina state Key laboratory of High-efficiency Utilization of Coal and Green Chemical engineering College of Chemistry&Chemical EngineeringNingxia UniversityYinchuan 750021NingxiaChina College of Chemistry&Chemical engineering Yan’an UniversityYan’an 716000ShaanxiChina School of Chemistry and Chemical engineering Shanghai Jiao Tong UniversityShanghai 200240China

Designing efficient and long-lasting non-metal electrocatalysts is an urgent task for addressing the issue of kinetic hysteresis in electrochemical oxidation reactions.The bimetallic hydroxides,catalyzing the oxygen evolution reaction(OER),have significant research potential because hydroxide reconstruction to generate an active phase is a remarkable advantage.Herein,the complete reconstruction of ultrathin CoNi(OH)_(2) nanosheets was achieved by embedding Ag nanoparticles into the hydroxide to induce a spontaneous redox reaction(SRR),forming heterojunction Ag@CoNi(OH)_(2) for bifunctional hydrolysis.Theoretical calculations and in situ Raman and ex situ characterizations revealed that the inductive effect of the Ag cation redistributed the charge to promote phase transformation to highly activate Ag-modified hydroxides.The Co-Ni dual sites in Co/NiOOH serve as novel active sites for optimizing the intermediates,thereby weakening the barrier formed by OOH^*.Ag@CoNi(OH)_(2) required a potential of 1.55 V to drive water splitting at a current density of 10 mA cm^(-2),with nearly 98.6% Faraday efficiency.Through ion induction and triggering of electron regulation in the OER via the synergistic action of the heterogeneous interface and surface reconstruction,this strategic design can overcome the limited capacity of bimetallic hydroxides and bridge the gap between the basic theory and industrialization of water decomposition.

关键词： Surface reconstruction Bimetallic hydroxides Ag nanoparticle Operando Raman Overall water splitting

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Top priority current path between SiC particles during ultra-high temperature flash sintering: Presence of PyC “bridges”

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Journal of Advanced Ceramics 2024年第2期13卷 255-262页

作者： Le Lu Tianlong Liu Zhaofeng Chen Fei Wang Mengmeng Yang Qiong Wu Lixia Yang Huanyong Li International laboratory for Insulation and Energy Efficiency materials College of Materials Science and TechnologyNanjing University of Aeronautics and AstronauticsNanjing 211106China state Key laboratory of Solidification Processing School of Materials and EngineeringNorthwestern Polytechnical UniversityXi’an 710072China

Flash sintering(FS)is a novel technique for rapidly densifying silicon carbide(SiC)ceramics.This work achieved a rapid sintering of SiC ceramics by the utilization of ultra-high temperature flash sintering within 60 s.Pyrolysis carbon(PyC)“bridges”were constructed between SiC particles through the carbonisation of phenolic resin,providing a large number of current channels.The incubation time of the flash sintering process was significantly reduced,and the sintering difference between the centre and the edge regions of the ceramics was minimized,with an average particle size of the centre region and edge region being 12.31 and 9.02μm,respectively.The results showed that the porosity of the SiC ceramics after the flash sintering was reduced to 14.79% with PyC“bridges”introduced,and the Vickers hardness reached 19.62 GPa.PyC“bridges”gradually evolved from amorphous eddy current carbon to oriented graphite carbon,indicating that the ultra-high temperature environment in which the sample was located during the flash sintering was successfully constructed.Ultra-high temperature flash sintering of SiC is expected to be applied to the local repair of matrix damage in SiC ceramic matrix composites.

关键词： silicon carbide(SiC) flash sintering(FS) pyrolytic carbon(PyC)"bridges" current path instantaneous

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